ELECTROCHIMICA ACTA
·
2023
·
IF 6.6
Baochun Wang,Haorong Chen,Zilong Wang,Zhaoqing Jin,Anbang Wang,Yaqin Huang,Weikun Wang
Lithium-sulfur batteries (LSBs) are promising candidates as next-generation secondary batteries due to their advantages with respect to cost and energy density. However, their practical application is hindered by their slow kinetics and the shuttle behavior of soluble polysulfide ions. Herein, we successfully prepared a three-dimensional porous conductive catalyst material with an atomic-level Ni–N 4 structure. The results showed that a strong adsorption of lithium polysulfides (LiPSs) by the Ni–N 4 catalytic active sites and a strong catalytic effect on the conversion of LiPSs in the sulfur reduction reaction (SRR) as well as the lithium sulfide oxidation reaction (SOR) were achieved, effectively inhibiting the shuttle effect of polysulfide ions and promoting the sulfur cathode kinetics process. Thus, the LSBs exhibited an excellent performance with a specific capacity of 829.8 mAh g –1 and an average coulombic efficiency of 98.8 % after 420 cycles at a high rate of 1 C. Our work provides new insights and novel efforts to solve the shuttle effect in LSBs.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Mingyue Xie,Yong Wu,Hao Gu,Yuhao Peng,Shan Zhang,Feng Ryan Wang,Wei Xiao,Dong Gu
Deuterated compounds have broad applications across various fields, with dehalogenative deuteration serving as an efficient method to obtain these molecules. However, the diverse electronic structures of active sites in the heterogeneous system and the limited recyclability in the homogeneous system significantly hinder the advancement of dehalogenative deuteration. In this study, we present a catalyst composed of copper single-atom sites anchored within an ordered mesoporous nitrogen-doped carbon matrix, synthesized via a mesopore confinement method. The Cu1/OMNC-1100 catalyst, characterized by Cu–N4 sites, demonstrates exceptional performance, high functional group tolerance, and remarkable durability in the deuteration of 2-bromo-6-methoxynaphthalene under relatively mild conditions (80 °C, 2 MPa of CO). Experimental results combined with X-ray absorption fine structure analysis reveal that Cu–N3 sites can be converted into more stable Cu–N4 counterparts at higher pyrolysis temperatures, resulting in enhanced catalytic activity. This work demonstrates a strategy for designing single-atom site catalysts with tunable coordination environments, providing a promising approach to improving catalytic performance in selective dehalogenative reactions under relatively mild conditions.
研究领域:
化学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 9
·4807-4815
·
IF 11.301
Ying Gu,Aiping Wu,Lei Wang,Dongxu Wang,Haijing Yan,Peng Yu,Ying Xie,Chungui Tian,Fanfei Sun,Honggang Fu
Single-atom catalysts (SACs) have been promising in various catalytic fields, but the controllable synthesis of SACs with high stability remains challenging. Here, we show a robust strategy toward the fabrication of highly efficient and stable SACs based on the “competitive occupancy” of two metal (M) species on graphene oxide (GO). The abundant M1 (Ti) species predominantly occupy more groups of GO, thereby leaving a tiny number of groups in the gaps of the M1 species to combine with M2 (Co2+, etc.) species. Consequently, this guarantees the formation of Co–N4 SACs embedded in 2D TiN/rGO sheets during nitridation. Further, TiN can act as a “spacer” to prevent Co–N4 from aggregation, thereby improving catalyst stability. Co–N4/TiN–rGO exhibits outstanding catalytic performance for the fast conversion of highly concentrated aromatic nitro compounds (∼0.3–2 mM) into amino compounds and excellent recyclability, which is the best among reported catalysts. In contrast, TiN/rGO has no obvious activity, and Co4N–rGO prepared without Ti competition shows poor activity and stability, which indicates the vital role of Co–N4 and TiN for obtaining the remarkable catalytic ability of Co–N4/TiN–rGO. The reaction mechanism is also proposed based on theoretical calculations. The strategy can be used to design Ni (Fe, Cr, Cu)-based SACs.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
ACS Nano
·
2025
·
IF 16
Xiao Ge,Xinya Liu,Jinze Xu,Xiyang Zheng,Li-jiao Tian,Xiaozhi Wang
Rational regulation of the coordination environment of single-atom catalysts (SACs) is a promising yet challenging strategy to enhance their activity. Here, we introduce an O atom into the second coordination shell of Co–N4 sites via a simple thermal treatment, forming a Co–N4–ON matrix to boost photosynthetic hydrogen peroxide (H2O2) production. This modification significantly alters the electronic structure of the Co site, bringing the d-band center closer to the Fermi energy and elevating the conduction band of Co–N4–CN to enhance its reducing capacity. Density functional theory (DFT) calculations reveal intensified charge redistribution and a reduced work function in Co–N4–ON, facilitating O2 adsorption. Notably, Co–N4–ON exhibits the lowest O2 adsorption energy, indicating a stronger interaction between Co–N4–O and O2, which is further strengthened by orbital hybridization and charge transfer at their interface, leading to enhanced O2 activation. The optimized Co–N4–ON catalyst demonstrates superior O2 reduction capabilities with the lowest energy barrier during H2O2 desorption. Consequently, it achieves a H2O2 production rate of 3098.18 μmol g–1 h–1 under neutral conditions, which is 2.6 times higher than that of Co–N4–CN. Moreover, it maintains a production rate of 1967.79 μmol g–1 h–1 over 10 h in a continuous flow reactor under natural sunlight and ambient air, highlighting its durability and practicality. This study underscores the crucial role of the second coordination shell in SACs and offers valuable insights into their atomic-level structure–activity relationships, thus contributing to advancements in catalyst design for efficient photosynthetic H2O2 production.
研究领域:
化学
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材料科学
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Zhengwen Fan,Xinjiao Cui,Jiankun Wei,Chan Chen,Haolin Tang,Junsheng Li
Fe N C is the most promising material to replace the noble metal catalyst for cathodic oxygen reduction reaction in proton exchange membrane fuel cells (PEMFCs). However, the practical performance of Fe N C catalyst is significantly limited by its low active site (Fe-N 4 ) density. Herein, we propose to promote the formation of Fe-N 4 active sites in Fe N C catalyst by strengthening the interaction of N precursors and Fe precursors during the carbonization synthesis. In our approach, ionic liquid (IL, [EMIM][NTf 2 ]) with high nitrogen content and good thermal stability is caged in the pores of Fe-ZIF-8 through the host–guest interactions. These interactions are critical for the preservation of Fe and N species and formation of active sites during the synthesis. The optimal catalyst developed with this approach (Fe 0.05 N C/10) has a high density of accessible Fe-N 4 sites (1.88*10 19 sites g −1 ). Therefore, in both acidic and alkaline media, Fe 0.05 N C/10 showed excellent ORR activity comparable to commercial Pt/C catalyst. Moreover, PEMFC performance with a peak power density of 300 mW cm −2 was demonstrated with Fe 0.05 N C/10 under H 2 /O 2 conditions. The synthetic approach reported herein may be used for tailoring of advanced catalyst with high intrinsic activity.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
·
2022
·Vol. 38
·期 5
·1232-1238
·
IF 2.726
Chen Weijie,Xia Huicong,Guo Kai,Jin Wangzhe,Du Yu,Yan Wenfu,Qu Gan,Zhang Jianan
Lithium-sulfur(Li-S) batteries have been puzzled by the “shuttle effect”. In the recent years, catalytic materials present a huge potential for solving this problem. However, the exploitation for catalytic activity was still challenging in Li-S batteries. In this article, we put forward a single atom catalyst (SAC) of FeN 4 coupled with Fe 3 C on the N-doped carbon (FeN 4 /Fe 3 C@NC) by one-step pyrolysis method. The FeN 4 and Fe 3 C synergistically catalyze the polysulfides conversion when the N-doped carbon provides the high conductive three-dimensional skeleton in Li-S batteries. As a result, the FeN 4 /Fe 3 C@NC shows a specific capacity of 1100 mA·h/g at 0.2 C(1 C=1675 mA/g). In addition, the FeN 4 /Fe 3 C@NC maintains 99.01% of the pristine specific capacity after 100 cycles at 0.5 C, indicating the improved electrochemical performance in Li-S batteries. This work sheds new lights on the design of engineering catalysts for developing high-performance Li-S batteries.
研究领域:
电化学
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能源材料
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纳米催化
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电池技术
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材料化学
✓ 已验证
DOI
高影响因子
ACS ES&T Engineering
·
2022
·
IF 0
Shuqian Dong,Xu Chen,Linfeng Su,Yingjie Wen,Yuechu Wang,Qihao Yang,Li Yi,Wenwen Xu,Qiu Yang,Peilei He,Yunqing Zhu,Zhiyi Lu
Photo-Fenton degradation as a promising strategy for antibiotic wastewater treatment attracted extensive attention, while the unsatisfactory catalytic performance vitally limits its industrial application. Herein, we demonstrate that confining atomically dispersed Cu into C3N4 (Cu–C3N4) enables fast H2O2 activation and efficient separation of photogenerated electron–hole pairs, resulting in a dramatic improvement of the degradation efficiency of the Photo-Fenton reaction. Photo-Fenton degradation of ciprofloxacin (CIP) was close to 99% within 30 min over optimized Cu–C3N4, corresponding to a pseudo-first-order rate constant of ∼0.0978 min–1, almost 4.5 times higher than pure C3N4 counterpart. The electron paramagnetic resonance, quenching experiments, and X-ray absorption fine structure results reveal that the superior Photo-Fenton catalytic performance is attributed to a nonradical reaction pathway, where the H2O2 is activated by the formation of the O═Cu–N4═O intermediate. The advanced catalyst as well as the refreshing H2O2 activation mechanism are of profound significance for the materials design in the wastewater treatment field.
研究领域:
环境科学
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材料科学
·
化学工程
✓ 已验证
DOI
GREEN CHEMISTRY
·
2025
·
IF 9.2
Shuling Liu,Tongjun Li,Guozheng Dong,Xinao Wei,Keke Zhao,Bangan Lu,Yu Chen,Yanyan Liu,Jianchun Jiang,Baojun Li
To develop low-cost and efficient oxygen reduction reaction (ORR) electrocatalysts, single-atom catalysts (SACs) have attracted great attention to become vital to the applications of zinc-air batteries (ZABs) because of their high catalytic activity. The development of integrated SACs as self-supporting electrodes is crucial for ZABs to overcome the drawback of powder catalysts requiring binder. Herein, an integrated atomically dispersed FeSA/NC catalyst was obtained by pyrolysis of Fe-containing ZIF-8 on fir wood-derived carbon. The atomically dispersed Fe-N4 is an efficient catalytic active site for ORR. The self-supported ordered porous structure and continuous conductive network of the catalyst provide favorable conditions for the rapid mass/electron transfer. FeSA/NC catalyst demonstrates a positive half-wave potential of 0.90 V in 0.1 M KOH electrolyte and 0.80 V in acidic solution. The outstanding ORR activity outperforms those of commercial Pt/C and most reported M-N-C (M=Fe, Co, Ni, etc.) catalysts. A quasi-solid-state ZAB using the FeSA/NC in cathode shows an excellent peak power density of 77 mW cm–2 at 121 mA cm–2. The performance in quasi-solid-state batteries exceeds that of most other catalysts. This work provides a new path to the catalytically active carbon via design of self-supporting SACs, and a clear demonstration of prospects in quasi-solid-state energy devices.
研究领域:
材料科学
·
电化学
·
能源技术
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2024
·
IF 15.7
Yuan Jiang,Ji Yang,Mu-Lin Li,Xue-Jia Wang,Na Yang,Wei-Ping Chen,Jin-Chao Dong,Jian-Feng Li
ABSTRACT Metal-nitrogen-carbon single-atom catalysts (M-N-C SACs) have emerged as a highly promising material for ammonia synthesis from electrocatalytic nitrate reduction due to their isolated metal site and capacity to prevent the N–N coupling. However, understanding the structure-activity relationship at molecular level remains challenging because of the inhomogeneous M N x structure presented in current synthesized M-N-C catalysts. In this study, we utilized metal phthalocyanine ( M Pc) as a model platform catalyst containing a uniform and well-defined M N 4 center to unravel their intrinsic activity tendency toward ammonia synthesis from nitrate reduction, both experimentally and theoretically. Our experimental results exhibit a significant activity difference for ammonia production in the order of FeN 4 > CuN 4 > NiN 4 > MnN 4 > CoN 4 > ZnN 4 , and among which the FeN 4 site delivers much higher faradic efficiency and the highest turnover frequency of 83.3% and 4395.2 h –1 at –1.0 V vs . RHE, respectively. Density-functional theory calculations indicates that, compared to CoN 4 and MnN 4 , the FeN 4 site not only has appropriate adsorption strength for NO x intermediate species, but also has certain inhibitory effects on hydrogen evolution reaction process. These findings provide systematic and reliable guidance for catalyst synthesis toward nitrate reduction to NH 3 from both the experimental and computational perspectives.
研究领域:
催化
·
电化学
·
材料科学
·
理论化学
✓ 已验证
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2025
·
IF 7.9
Lihui Xiao,Yaqiang Li,Peixia Yang,Qiang Lv,Xiangyu Lu,Hao Xu,Ruopeng Li,Huiling Zhang,Shengbo Yang,Anmin Liu,Dan Wang,Jinqiu Zhang,Maozhong An
Carbon nanotubes' (CNTs) preparation and formation mechanisms are of great interest. To improve their performance in the oxygen reduction reaction (ORR), a post-treatment to add active centers is required. This study presents a simple method using a molten-salt template to self-assemble bamboo-shaped CNTs (B-Fe-N-C) with highly stable Fe-N 4 (Fe-pyridinic-N 4 ) sites. By analyzing the evolution of high-temperature materials and the intermolecular bonding process, the formation mechanism of B-Fe-N-C follows a two-dimensional material synthesis--bonding--self-assembly--growth mechanism. Impressively, B-Fe-N-C exhibits superior ORR performance (a half-wave potential of 0.868 V) and stability (only 3 mV attenuation after 10000 cycles of accelerated durability test) in alkaline medium. Density functional theory calculations demonstrate that Fe-Pyridinic-N 4 sites can lower the energy barrier for ORR. Furthermore, Comsol multiphysics simulations confirm the significant enhancement of oxygen mass transfer by bamboo-shaped B-Fe-N-C. Therefore, B-Fe-N-C is employed in zinc-air batteries, resulting in nice discharge performance and high peak power density.
研究领域:
材料科学
·
电化学
·
理论计算
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Dan Xu,Ruirui Liu,Jianfeng Li,Huacheng Zhao,Jiantai Ma,Zhengping Dong
Transfer hydrogenation reactions using non-noble metal-based nanocatalysts are extensively attractive due to their low-cost and green reaction conditions. But construction of such catalysts with maximum metal atom efficiency and high catalytic activity is still a challenging research goal. Here, atomically dispersed Co catalysts with Co-N 4 active sites were fabricated, which builds a bridge for transfer hydrogenation between nitroarenes and saturated N-heterocycles in aqueous solution. The TOF value of the transfer hydrogenation reaction is much higher than nanoparticle catalyst for this reaction. Density functional theory (DFT) calculations and control experiments reveal that the excellent performance origins from the Co-N 4 sites, which combines the dehydrogenation of 1,2,3,4-tetrahydroquinoline with hydrogenation of nitrobenzene in one-pot. This work not only has an in-depth understanding of active sites but also shows a unique activity to the challenging, highly efficient, and green transfer hydrogenation reaction.
研究领域:
催化化学
·
材料科学
·
理论化学
✓ 已验证
DOI
高影响因子
ANALYTICAL BIOCHEMISTRY
·
2021
·
IF 3.365
Yan-Ying Xu,Fei Qin,Yi-Xin Dai,Xue-Feng Zhong,Juan Yan,Su-Mei Xu,Ping-Sheng Xu
This study aimed to develop an LC-MS/MS method for determining sildenafil and its metabolites N -desmethylsildenafil and N1,N4 -desmethylsildenafil in human plasma and applying it to a pharmacokinetic study of sildenafil in healthy volunteers. Sildenafil-d8 was used as the internal standard. Plasma samples were pretreated via protein precipitation with acetonitrile . The extractives were then separated on an ACQUITY UPLC BEH C18 (50-mm × 2.1-mm, 1.7-μm) column using gradient elution . The aqueous and organic mobile phases were ammonium formate 2 mM supplemented with 0.1% formic acid in water and acetonitrile, respectively, and the flow rate was 0.3 mL/min. An electrospray ionization source was applied, and multiple reaction monitoring was operated in the positive mode with selective channels at m / z 475.30 → 100.10, 461.20 → 283.30, 483.30 → 108.10, and 449.00 → 283.00 for sildenafil, sildenafil-d8, N - desmethylsildenafil, and N1,N4 -desmethylsildenafil, respectively. The linear calibration curves of sildenafil and its metabolites spanned 1.0–1000 ng/mL. The lower limit of quantification was 1.0 ng/mL. The extractive recovery of analytes from the biological matrix was more than 90% and the matrix effect complied with relevant provisions. The intra- and inter-day precisions of sildenafil and its metabolite were <10%. The intra- and inter-day accuracy of sildenafil, N - desmethylsildenafil, and N1,N4 -desmethylsildenafil was more than 99%. The method is highly sensitive and selective, and it was successfully applied to the bioequivalence studies of 100-mg sildenafil citrate tablets in 40 healthy Chinese volunteers.
研究领域:
药物分析
·
临床药理学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）